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Title: Covalently Bound Nitroxyl Radicals in an Organic Framework

Abstract

A series of covalent organic framework (COF) structures is synthesized that possesses a tunable density of covalently bound nitroxyl radicals within the COF pores. The highest density of organic radicals produces an electron paramagnetic resonance (EPR) signal that suggests the majority of radicals strongly interact with other radicals, whereas for smaller loadings the EPR signals indicate the radicals are primarily isolated but with restricted motion. The dielectric loss as determined from microwave absorption of the framework structures compared with an amorphous control suggests that free motion of the radicals is inhibited when more than 25% of available sites are occupied. The ability to tune the mode of radical interactions and the subsequent effect on redox, electrical, and optical characteristics in a porous framework may lead to a class of structures with properties ideal for photoelectrochemistry or energy storage.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); NREL Laboratory Directed Research and Development (LDRD)
OSTI Identifier:
1326170
Report Number(s):
NREL/JA-5900-67035
Journal ID: ISSN 1948-7185
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 18; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; covalent organic framework; conductivity; organic radical

Citation Formats

Hughes, Barbara K., Braunecker, Wade A., Bobela, David C., Nanayakkara, Sanjini U., Reid, Obadiah G., and Johnson, Justin C. Covalently Bound Nitroxyl Radicals in an Organic Framework. United States: N. p., 2016. Web. doi:10.1021/acs.jpclett.6b01711.
Hughes, Barbara K., Braunecker, Wade A., Bobela, David C., Nanayakkara, Sanjini U., Reid, Obadiah G., & Johnson, Justin C. Covalently Bound Nitroxyl Radicals in an Organic Framework. United States. https://doi.org/10.1021/acs.jpclett.6b01711
Hughes, Barbara K., Braunecker, Wade A., Bobela, David C., Nanayakkara, Sanjini U., Reid, Obadiah G., and Johnson, Justin C. 2016. "Covalently Bound Nitroxyl Radicals in an Organic Framework". United States. https://doi.org/10.1021/acs.jpclett.6b01711.
@article{osti_1326170,
title = {Covalently Bound Nitroxyl Radicals in an Organic Framework},
author = {Hughes, Barbara K. and Braunecker, Wade A. and Bobela, David C. and Nanayakkara, Sanjini U. and Reid, Obadiah G. and Johnson, Justin C.},
abstractNote = {A series of covalent organic framework (COF) structures is synthesized that possesses a tunable density of covalently bound nitroxyl radicals within the COF pores. The highest density of organic radicals produces an electron paramagnetic resonance (EPR) signal that suggests the majority of radicals strongly interact with other radicals, whereas for smaller loadings the EPR signals indicate the radicals are primarily isolated but with restricted motion. The dielectric loss as determined from microwave absorption of the framework structures compared with an amorphous control suggests that free motion of the radicals is inhibited when more than 25% of available sites are occupied. The ability to tune the mode of radical interactions and the subsequent effect on redox, electrical, and optical characteristics in a porous framework may lead to a class of structures with properties ideal for photoelectrochemistry or energy storage.},
doi = {10.1021/acs.jpclett.6b01711},
url = {https://www.osti.gov/biblio/1326170}, journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 18,
volume = 7,
place = {United States},
year = {Thu Sep 15 00:00:00 EDT 2016},
month = {Thu Sep 15 00:00:00 EDT 2016}
}